Optical signatures of coherence in molecular dimers

Abstract

We calculate experimentally measurable signatures of quantum correlations in a coupled molecular dimer that strongly interacts with its vibrational environment. We investigate intensity and mode-resolved photon coincidences for different relative orientations of such dimers and observe spatio-temporal correlations for various configurations. We find that projective measurements can produce cooperative signatures even when emitters are arranged orthogonal to each other. To model effects of vibrational environments that are present in realistic experimental situations, we use the polaron framework. Furthermore, we also account for the effects of finite instrument response, varying temperature, and the presence of static disorder. We analyze the effect of disorder in both dimer orientation and measurement direction and find that photon coincidences remain well-resolvable using state-of-the-art detectors. This work enhances our understanding of cooperative emission from two coupled emitters and offers direction for future experiments on probing their coherent dynamics.